Controlling Nonsequential Double Ionization in Two-Color Circularly Polarized Femtosecond Laser Fields

Mancuso, Christopher; Dorney, Kevin M.; Hickstein, Daniel D.; Chaloupka, J. L.; Ellis, Jennifer L.; Dollar, F.; Knut, Ronny; Grychtol, Patrik; Zusin, Dmitriy; Gentry, Christian; Gopalakrishnan, Maithreyi; Kapteyn, Henry C.; Murnane, Margaret M.

doi:10.1103/physrevlett.117.133201

Cited by 119 publications

(61 citation statements)

References 57 publications

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“…The results from the CE simulations allow us to recognize that the observed ionization enhancement in counter-rotating fields is an indication of returning electron trajectories for single ionization, just as the observation of the familiar "knee" in nonsequential double ionization [79] for counter-rotating fields [34] is a signature of returning electron trajectories for double ionization. This similarity is notable as the strength of the electronion interaction is much different between the two processes.…”

Section: Figmentioning

confidence: 93%

“…For an expanded description of how the model was employed see the Supplemental Material of Ref. [34]. Remarkably, even though these simulations are purely classical and do not include any quantum effects, an ionization enhancement is still observed in counterrotating fields for a wide range of IB/IR ratios [ Fig.…”

Section: Iiic Classical Ensemble Simulationsmentioning

confidence: 99%

“…phase matched) source of circularly polarized EUV [23][24][25][26][27][28][29] and soft X-ray [30] beams with sufficient flux for applications in magnetic spectroscopies of materials [28,30]. In the case of SFI, bicircular fields allow electrons to be driven in 2D trajectories prior to rescattering from the parent ion [31][32][33][34][35][36][37][38]. Interestingly, the shape of the bicircular waveform -and therefore the physics of the HHG and SFI processes -can be modified by changing the relative wavelengths, intensities, and ellipticities of the two driving fields [29][30][31]36].…”

Section: Introductionmentioning

confidence: 99%

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Observation of ionization enhancement in two-color circularly polarized laser fields

et al. 2017

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When atoms are irradiated by two-color circularly polarized laser fields the resulting strong field processes are dramatically different than when the same atoms are irradiated by a single-color ultrafast laser. For example, electrons can be driven in complex 2D trajectories before rescattering or circularly polarized high harmonics can be generated, which was once thought impossible. Here, we show that two-color circularly polarized lasers also enable control over the ionization process itself and make a surprising finding: the ionization rate can be enhanced by up to 700% simply by switching the relative helicity of the two-color circularly polarized laser field. This enhancement is experimentally observed in helium, argon and krypton over a wide range of intensity ratios of the twocolor field. We use a combination of advanced quantum and fully classical calculations to explain this ionization enhancement as resulting in part due to the increased density of excited states available for resonance-enhanced ionization in counter-rotating fields compared with co-rotating fields. In the future, this effect could be used to probe the excited state manifold of complex molecules.

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Section: Figmentioning

confidence: 93%

Section: Iiic Classical Ensemble Simulationsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Observation of ionization enhancement in two-color circularly polarized laser fields

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“…Control of electron-electron correlation in double ionization in atoms has been demonstrated through the free parameters Δt and E 2ω of OTC laser fields [38][39][40][41][42][43]. The time-delay between the laser fields can significantly affect the time and the distance of the closest approach of the returning electron [11].…”

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confidence: 99%

Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

2017

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We demonstrate the control of electron-electron correlation in frustrated double ionization (FDI) of the two-electron triatomic molecule D + 3 when driven by two orthogonally polarized two-color laser fields. We employ a three-dimensional semi-classical model that fully accounts for the electron and nuclear motion in strong fields. We analyze the FDI probability and the distribution of the momentum of the escaping electron along the polarization direction of the longer wavelength and more intense laser field. These observables when considered in conjunction bear clear signatures of the prevalence or absence of electron-electron correlation in FDI, depending on the time-delay between the two laser pulses. We find that D + 3 is a better candidate compared to H 2 for demonstrating also experimentally that electron-electron correlation indeed underlies FDI.PACS numbers: 33.80. Rv, 34.80.Gs, 42.50.Hz Frustrated double ionization (FDI) is a major process in the nonlinear response of multi-center molecules when driven by intense laser fields, accounting roughly for 10% of all ionization events [1,2]. In frustrated ionization an electron first tunnel-ionizes in the driving laser field. Then, due to the electric field of the laser pulse, it is recaptured by the parent ion in a Rydberg state [3]. This process is a candidate for the inversion of N 2 in free-space air lasing [4]. In FDI an electron escapes and another one occupies a Rydberg state at the end of the laser pulse. In theoretical studies of strongly-driven two-electron diatomic and triatomic molecules, two pathways of FDI have been identified [2,8]. Electron-electron correlation is important, primarily, for one of the two pathways. It is well accepted that electron-electron correlation underlies a significant part of double ionization in strongly-driven molecules-a mechanism known as non-sequential double ionization [9,10]. However, electron-electron correlation in FDI has yet to be accessed experimentally.Here, we propose a road for future experiments to identify the important role of electron-electron correlation in FDI. We identify the parameters of orthogonally polarized two-color (OTC) laser fields that best control the relevant pathway for electron-electron correlation in FDI. We demonstrate traces of attosecond control of electron motion in space and time in two observables of FDI as a function of the time-delay between the fundamental 800 nm and the second harmonic 400 nm laser field. We show that, together, the FDI probability and the momentum of the escaping electron along the fundamental laser field bear clear signatures of the turning on and off of electronelectron correlation.Two-color laser fields are an efficient tool for controlling electron motion [11,12] and for steering the outcome of chemical reactions [13][14][15]. Other applications include the field-free orientation of molecules [16][17][18], the generation of high-harmonic spectra [19][20][21][22] and probing atomic and molecular orbital symmetry [23][24][25]. The strongly-driven dynam...

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“…Ultrashort bichromatic laser fields have emerged as a new twist to coherently control ultrafast electron dynamics in atoms [1][2][3][4][5][6], molecules [7][8][9] and solids [10][11][12]. In recent years, (ω : 2ω)-fields have been employed in numerous applications to observe and manipulate the motion of electron wave packets on their intrinsic timescales.…”

Section: Introductionmentioning

confidence: 99%

Ultrashort polarization-tailored bichromatic fields from a CEP-stable white light supercontinuum

et al. 2017

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We apply ultrafast polarization shaping to an ultrabroadband carrier envelope phase (CEP) stable white light supercontinuum to generate polarization-tailored bichromatic laser fields of low-order frequency ratio. The generation of orthogonal linearly and counter-rotating circularly polarized bichromatic fields is achieved by introducing a composite polarizer in the Fourier plane of a 4 f polarization shaper. The resulting Lissajous-and propeller-type polarization profiles are characterized experimentally by cross-correlation trajectories. The scheme provides full control over all bichromatic parameters and allows for individual spectral phase modulation of both colors. Shaper-based CEP control and the generation of tailored bichromatic fields is demonstrated. These bichromatic CEP-stable polarization-shaped ultrashort laser pulses provide a versatile class of waveforms for coherent control experiments.

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Controlling Nonsequential Double Ionization in Two-Color Circularly Polarized Femtosecond Laser Fields

Cited by 119 publications

References 57 publications

Observation of ionization enhancement in two-color circularly polarized laser fields

Observation of ionization enhancement in two-color circularly polarized laser fields

Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

Ultrashort polarization-tailored bichromatic fields from a CEP-stable white light supercontinuum

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